In this paper, we present first insights on the rapid large-scale self-assembly of monocrystalline Au nano-islands produced at the Nanotechnology Research Laboratory (ANU) and their application as efficient LSPR surfaces. Our one-step deposition method by in-situ coalescence of hot nanoparticle aerosols produces a discontinuous monolayer of highly-faceted monocrystals. These findings provide a very rapid, low-cost nanofabrication tool for the engineering of highly homogenous Au metasurfaces. Applications of these new metasurfaces range from ultra-sensitive optical gas sensors to photocatalytic macro-reactors.